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Space-Confined Self-Regulation Mechanism from a Capsule Catalyst to Realize an Ethanol Direct Synthesis Strategy
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-01-03 , DOI: 10.1021/acscatal.9b02891 Peng Lu 1, 2 , Qingjun Chen 1 , Guohui Yang 1, 3 , Li Tan 1 , Xiaobo Feng 1 , Jie Yao 1 , Yoshiharu Yoneyama 1 , Noritatsu Tsubaki 1, 4
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-01-03 , DOI: 10.1021/acscatal.9b02891 Peng Lu 1, 2 , Qingjun Chen 1 , Guohui Yang 1, 3 , Li Tan 1 , Xiaobo Feng 1 , Jie Yao 1 , Yoshiharu Yoneyama 1 , Noritatsu Tsubaki 1, 4
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A capsule catalyst, being composed of a catalytic zeolite membrane and a catalyst core, can accomplish multiple catalysis reactions or several organic synthesis reactions in a single step, enhancing energy efficiency, erasing unnecessary separation engineering, and creating many unexpected synergistic effects via tandem catalysis. This report discloses an ethanol synthesis strategy from syngas (CO + H2) and syngas-derived dimethyl ether (DME) by a tailor-made catalyst with a macroscopic capsule structure. The macroscopically designed capsule catalyst consisted of a millimeter-sized Cu/ZnO core and a micrometer-sized H-Mordenite zeolite shell. The catalyst preparation process further successfully fabricated a zeolite shell, migrated a few Cu from the core, as the promoter of the shell, to significantly improve the catalyst performance. As the methanol byproduct can be easily recycled to DME as a reactant via a simple dehydration reaction, ethanol selectivity can reach 100% theoretically. It is demonstrated that a space-confined-self-regulation mechanism derived from a macroscopic capsule structure serves as a multifunctional switch to manipulate tandem reactions: arranging reaction steps in a favorable order and depressing side reactions simultaneously. These findings will inspire designing a heterogeneous catalyst with multiple functions, shortening the organic or catalytic synthesis route, and also open an avenue to ethanol synthesis from syngas, as DME is also simply produced from syngas.
中文翻译：
胶囊催化剂的空间限制自我调节机制实现乙醇直接合成策略
由催化沸石膜和催化剂核组成的胶囊催化剂可在一个步骤中完成多个催化反应或多个有机合成反应，从而提高能源效率，消除不必要的分离工程，并通过串联催化产生许多意想不到的协同效应。该报告公开了由合成气（CO + H 2）和合成气衍生的二甲醚（DME），该催化剂是量身定制的具有宏观胶囊结构的催化剂。宏观设计的胶囊催化剂由毫米大小的Cu / ZnO核和微米大小的H-丝光沸石沸石壳组成。催化剂的制备过程进一步成功地制备了沸石壳，从核中迁移出一些铜作为壳的促进剂，从而显着提高了催化剂的性能。由于甲醇副产物可以通过简单的脱水反应轻松地作为反应物循环回DME，因此乙醇的选择性理论上可以达到100％。证明了从宏观胶囊结构派生的空间限制自我调节机制可作为操纵串联反应的多功能开关：以有利的顺序排列反应步骤并同时抑制副反应。这些发现将启发设计具有多种功能的非均相催化剂，缩短有机或催化合成路线，并为从合成气合成乙醇提供了途径，因为DME也是由合成气简单生产的。
更新日期：2020-01-04
中文翻译：
胶囊催化剂的空间限制自我调节机制实现乙醇直接合成策略
由催化沸石膜和催化剂核组成的胶囊催化剂可在一个步骤中完成多个催化反应或多个有机合成反应，从而提高能源效率，消除不必要的分离工程，并通过串联催化产生许多意想不到的协同效应。该报告公开了由合成气（CO + H 2）和合成气衍生的二甲醚（DME），该催化剂是量身定制的具有宏观胶囊结构的催化剂。宏观设计的胶囊催化剂由毫米大小的Cu / ZnO核和微米大小的H-丝光沸石沸石壳组成。催化剂的制备过程进一步成功地制备了沸石壳，从核中迁移出一些铜作为壳的促进剂，从而显着提高了催化剂的性能。由于甲醇副产物可以通过简单的脱水反应轻松地作为反应物循环回DME，因此乙醇的选择性理论上可以达到100％。证明了从宏观胶囊结构派生的空间限制自我调节机制可作为操纵串联反应的多功能开关：以有利的顺序排列反应步骤并同时抑制副反应。这些发现将启发设计具有多种功能的非均相催化剂，缩短有机或催化合成路线，并为从合成气合成乙醇提供了途径，因为DME也是由合成气简单生产的。
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